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Title: Lignin Depolymerization with Nitrate-Intercalated Hydrotalcite Catalysts

Journal Article · · ACS Catalysis
 [1];  [1];  [1];  [1];  [1];  [2];  [3];  [4];  [1];  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States). National Bioenergy Center
  2. National Renewable Energy Lab. (NREL), Golden, CO (United States). Hydrogen and Transportation Systems Center
  3. Shell Global Solutions, Inc., Houston, TX (United States). Shell Technology Center
  4. Shell Global Solutions, Inc., Amsterdam (Netherlands). Shell Technology Center

Hydrotalcites (HTCs) exhibit multiple adjustable parameters to tune catalytic activity, including interlayer anion composition, metal hydroxide layer composition, and catalyst preparation methods. Here in this paper, we report the influence of several of these parameters on β-O-4 bond scission in a lignin model dimer, 2-phenoxy-1-phenethanol (PE), to yield phenol and acetophenone. We find that the presence of both basic and NO3– anions in the interlayer increases the catalyst activity by 2–3-fold. In contrast, other anions or transition metals do not enhance catalytic activity in comparison to blank HTC. The catalyst is not active for C–C bond cleavage on lignin model dimers and has no effect on dimers without an α-OH group. Most importantly, the catalyst is highly active in the depolymerization of two process-relevant lignin substrates, producing a significant amount of low-molecular-weight aromatic species. The catalyst can be recycled until the NO3– anions are depleted, after which the activity can be restored by replenishing the NO3– reservoir and regenerating the hydrated HTC structure. These results demonstrate a route to selective lignin depolymerization in a heterogeneous system with an inexpensive, earth-abundant, commercially relevant, and easily regenerated catalyst.

Research Organization:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office (BETO)
Grant/Contract Number:
AC36-08GO28308
OSTI ID:
1238322
Report Number(s):
NREL/JA-5100-65864
Journal Information:
ACS Catalysis, Vol. 6, Issue 2; ISSN 2155-5435
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 55 works
Citation information provided by
Web of Science

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Recent advances on the utilization of layered double hydroxides (LDHs) and related heterogeneous catalysts in a lignocellulosic-feedstock biorefinery scheme journal January 2017
BINAP-copper supported by hydrotalcite as an efficient catalyst for the borrowing hydrogen reaction and dehydrogenation cyclization under water or solvent-free conditions journal January 2018
Highly selective cleavage C–O ether bond of lignin model compounds over Ni/CaO–H-ZSM-5 in ethanol journal March 2019
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Pseudomonas mendocina : Versatile Remediator from a Versatile Genus book December 2019
Catalytic Processes For Lignin Valorization into Fuels and Chemicals (Aromatics) journal June 2019
Valorization of Lignin by Partial Wet Oxidation Using Sustainable Heteropoly Acid Catalysts journal September 2017
Heterogeneously catalyzed lignin depolymerization journal June 2016
Oxidized demethylated lignin as a bio-based adhesive for wood bonding text January 2020
Gold-catalyzed conversion of lignin to low molecular weight aromatics journal January 2018
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